Enhanced Sampling of Crystal Nucleation with Graph Representation Learnt Variables.

Abstract

In this study, we present a graph neural network (GNN)-based learning approach using an autoencoder setup to derive low-dimensional variables from features observed in experimental crystal structures. These variables are then biased in enhanced sampling to observe state-to-state transitions and reliable thermodynamic weights. In our approach, we used simple convolution and pooling methods. To verify the effectiveness of our protocol, we examined the nucleation of various allotropes and polymorphs of iron and glycine in their molten states. Our graph latent variables, when biased in well-tempered metadynamics, consistently show transitions between states and achieve accurate thermodynamic rankings in agreement with experiments, both of which are indicators of dependable sampling. This underscores the strength and promise of our GNN variables for improved sampling. The protocol shown here should be applicable for other systems and other sampling methods.